Argon nucleation in a cryogenic supersonic nozzle

Argon nucleation in a cryogenic supersonic nozzle
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DOI:
10.1063/1.3299273
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发表时间:
2010-02-14
影响因子:
4.4
通讯作者:
Wyslouzil, Barbara
Wyslouzil, Barbara
中科院分区:
化学2区
文献类型:
--
作者:
Sinha, Somnath;Bhabhe, Ashutosh;Wyslouzil, Barbara

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我们在一个低温超音速喷管装置中测量了对应于氩的最大成核速率的压力p和温度T,估计的成核速率为J=10(17 +/- 1)cm(-3)s(-1)。当温度从34 K增加到53 K时,p从0.47 kPa增加到8 kPa。在这些条件下,经典成核理论预测的成核速率比观察到的速率低11-13个数量级,而平均场动力学成核理论预测的观察到的速率在1个数量级内。当前数据集似乎与Iland [J. Chem. Phys. 127,154506(2007)]在低温成核脉冲室中的测量一致。结合这两个数据集表明,经典的成核理论失败,因为它高估了临界团簇的大小和临界团簇的过剩内能。
We have measured pressures p and temperatures T corresponding to the maximum nucleation rate of argon in a cryogenic supersonic nozzle apparatus where the estimated nucleation rates are J=10(17 +/- 1) cm(-3) s(-1). As T increases from 34 to 53 K, p increases from 0.47 to 8 kPa. Under these conditions, classical nucleation theory predicts nucleation rates of 11-13 orders of magnitude lower than the observed rates while mean field kinetic nucleation theory predicts the observed rates within 1 order of magnitude. The current data set appears consistent with the measurements of Iland [J. Chem. Phys. 127, 154506 (2007)] in the cryogenic nucleation pulse chamber. Combining the two data sets suggests that classical nucleation theory fails because it overestimates both the critical cluster size and the excess internal energy of the critical clusters.